Numerical prediction of absolute crystallization rates in hard-sphere colloids.

Special computational techniques are required to compute absolute crystal nucleation rates of colloidal suspensions. Using crystal nucleation of hard-sphere colloids as an example, we describe in some detail the novel computational tools that are needed to perform such calculations. In particular, we focus on the definition of appropriate order parameters that distinguish liquid from crystal, and on techniques to compute the kinetic prefactor that enters in the expression for the nucleation rate. In addition, we discuss the relation between simulation results and theoretical predictions based on classical nucleation theory.

[1]  D. Frenkel,et al.  Prediction of absolute crystal-nucleation rate in hard-sphere colloids , 2001, Nature.

[2]  T. Palberg.  Crystallization kinetics of repulsive colloidal spheres , 1999 .

[3]  Medina-Noyola.  Long-time self-diffusion in concentrated colloidal dispersions. , 1988, Physical review letters.

[4]  David Chandler,et al.  Transition path sampling: throwing ropes over rough mountain passes, in the dark. , 2002, Annual review of physical chemistry.

[5]  Daan Frenkel,et al.  Suppression of crystal nucleation in polydisperse colloids due to increase of the surface free energy , 2001, Nature.

[6]  K. Hinsen,et al.  Dynamic computer simulation of concentrated hard sphere suspensions: I. Simulation technique and mean square displacement data , 1990 .

[7]  J. McTague,et al.  Should All Crystals Be bcc? Landau Theory of Solidification and Crystal Nucleation , 1978 .

[8]  David Chandler,et al.  Statistical mechanics of isomerization dynamics in liquids and the transition state approximation , 1978 .

[9]  H. Reiss,et al.  Some fundamental statistical mechanical relations concerning physical clusters of interest to nucleation theory , 1999 .

[10]  D. Frenkel,et al.  Can stacking faults in hard-sphere crystals anneal out spontaneously? , 1999 .

[11]  D. Frenkel,et al.  Solid-liquid interfacial free energy of small colloidal hard-sphere crystals , 2003 .

[12]  Berend Smit,et al.  Understanding Molecular Simulations: from Algorithms to Applications , 2002 .

[13]  W. Russel,et al.  Measurement of the hard-sphere equation of state using screened charged polystyrene colloids. , 1996, Physical review. B, Condensed matter.

[14]  J. P. van der Eerden,et al.  Science and technology of crystal growth , 1995 .

[15]  W. V. Megen,et al.  Crystallisation and the glass transition in suspensions of hard colloidal spheres , 1995 .

[16]  Palberg,et al.  Observation of Oriented Close-Packed Lattice Planes in Polycrystalline Hard-Sphere Solids. , 1998, Journal of colloid and interface science.

[17]  Direct calculation of the hard-sphere crystal /Melt interfacial free energy , 2000, Physical review letters.

[18]  Klein,et al.  Crystalline nucleation in deeply quenched liquids. , 1986, Physical review letters.

[19]  STACKING ENTROPY OF HARD-SPHERE CRYSTALS , 1998, cond-mat/9810287.

[20]  W. Meyer,et al.  Crystallization of hard-sphere colloids in microgravity , 1997, Nature.

[21]  P. Pusey,et al.  Phase behaviour of concentrated suspensions of nearly hard colloidal spheres , 1986, Nature.

[22]  Finite-size corrections to the free energies of crystalline solids , 1999, cond-mat/9909162.

[23]  P. Steinhardt,et al.  Bond-orientational order in liquids and glasses , 1983 .

[24]  Underwood,et al.  Glass transition in colloidal hard spheres: Measurement and mode-coupling-theory analysis of the coherent intermediate scattering function. , 1994, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[25]  Bartlett,et al.  Structure of crystals of hard colloidal spheres. , 1989, Physical review letters.

[26]  W. V. Megen,et al.  Crystallization kinetics of suspensions of hard colloidal spheres , 1997 .

[27]  M. J. Ruiz-Montero,et al.  Numerical evidence for bcc ordering at the surface of a critical fcc nucleus. , 1995, Physical review letters.

[28]  Berend Smit,et al.  Understanding molecular simulation: from algorithms to applications , 1996 .

[29]  J. W. Jansen,et al.  Light scattering of colloidal dispersions in non-polar solvents at finite concentrations. Silic spheres as model particles for hard-sphere interactions , 1983 .

[30]  Daan Frenkel,et al.  Numerical calculation of the rate of homogeneous gas–liquid nucleation in a Lennard-Jones system , 1999 .

[31]  C. Geyer,et al.  Annealing Markov chain Monte Carlo with applications to ancestral inference , 1995 .

[32]  Daan Frenkel,et al.  COMPUTER-SIMULATION STUDY OF FREE-ENERGY BARRIERS IN CRYSTAL NUCLEATION , 1992 .

[33]  K. Hall.  Another Hard‐Sphere Equation of State , 1972 .

[34]  G. Torrie,et al.  Monte Carlo free energy estimates using non-Boltzmann sampling: Application to the sub-critical Lennard-Jones fluid , 1974 .

[35]  Alfons van Blaaderen,et al.  Real-Space Structure of Colloidal Hard-Sphere Glasses , 1995, Science.

[36]  Ackerson,et al.  Density fluctuations during crystallization of colloids. , 1993, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[37]  Wilson C. K. Poon,et al.  Direct observation of pre-critical nuclei in a metastable hard-sphere fluid , 2001 .

[38]  William G. Hoover,et al.  Melting Transition and Communal Entropy for Hard Spheres , 1968 .